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Highly Sensitive Ammonia Gas Sensors at Room Temperature Based on the Catalytic Mechanism of N,C Coordinated Ni Single-Atom Active Center

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Nano-Micro Letters 2024年第12期16卷 515-531页

作者： Wenjing Quan Jia Shi Min Zeng Wen Lv Xiyu Chen Chao Fan Yongwei Zhang Zhou Liu Xiaolu Huang Jianhua Yang Nantao Hu Tao Wang Zhi Yang National Key Laboratory of Advanced Micro and Nano Manufacture Technology Shanghai Jiao Tong UniversityShanghai 200240People’s Republic of China Department of Micro/Nano Electronics School of Electronic Information and Electrical EngineeringShanghai Jiao Tong UniversityShanghai 200240People’s Republic of China Shanghai Key Laboratory of Intelligent Sensing and Detection Technology School of Mechanical and Power EngineeringEast China University of Science and TechnologyShanghai 200237People’s Republic of China

Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption properties to achieve highly sensitive and selective NH3 gas ***,Ni singleatom active sites based on N,C coordination(Ni-N-C)were interfacially confined on the surface of two-dimensional(2D)MXene nanosheets(Ni-N-C/Ti_(3)C_(2)Tx),and a fully flexible gas sensor(MNPE-Ni-N-C/Ti_(3)C_(2)Tx)was *** sensor demonstrates a remarkable response value to 5 ppm NH3(27.3%),excellent selectivity for NH3,and a low theoretical detection limit of 12.1 *** analysis by density functional calculation reveals that the Ni single-atom center with N,C coordination exhibits specific targeted adsorption properties for ***,its catalytic activation effect effectively reduces the Gibbs free energy of the sensing elemental reaction,while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas-solid *** sensor has a dual-channel sensing mechanism of both chemical and electronic sensitization,which facilitates efficient electron transfer to the 2D MXene conductive network,resulting in the formation of the NH3 gas molecule sensing ***,the passivation of MXene edge defects by a conjugated hydrogen bond network enhances the long-term stability of MXene-based electrodes under high humidity *** work achieves highly sensitive room-temperature NH3 gas detection based on the catalytic mechanism of Ni single-atom active center with N,C coordination,which provides a novel gas sensing mechanism for room-temperature trace gas detection research.

关键词： Gas sensor Single atom Catalytic activation targeted adsorption End-sealing passivation

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